Supramolecular chemistry has gained considerable attention since Nobel Prize awarding in 1987, where molecular recognition and assembly based on macrocyclic receptors play a great role. Much of supramolecular chemistry has sprung from designing novel macrocycles with specific selectivity and sensing function. And also, the ultimate goal of supramolecular chemistry is to construct higher-order architectures reversibly, achieving the special physical/chemical functions. Despite impressive development of macrocyclic chemistry in recent years, it is still a challenge to develop the building strategies leading to function-directed nanoarchitectures. With this regard, we systematically investigated the selective recognition/sensing and thermodynamic origins of macrocyclic receptors, and proposed two new building strategies of “modularization assembly” and “host-guest induced aggregation”. As a result, a series of stimuli-responsive assemblies were fabricated, showing potential applications in gene/drug delivery, molecular wire, and gas sensor. All these works contribute significantly to the development of functional supramolecular chemistry. In this project, we have published 105 SCI papers, totally cited over 2000 times. Our research work has obtained extensive attention from both national and international peer experts, and possesses scientific significance for supramolecular chemistry and other related disciplines.